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When two-dimensional (2D) group-VI transition metal dichalcogenides such as tungsten disulfide (WS2) are grown by atomic layer deposition (ALD) for atomic growth control at low deposition temperatures (≤450 °C), they often suffer from a nanocrystalline grain structure limiting the carrier mobility. The crystallinity and monolayer thickness control during ALD of 2D materials is determined by the nucleation mechanism, which is currently not well understood. Here, we propose a qualitative model for the WS2nucleation behavior on dielectric surfaces during plasma-enhanced (PE-) ALD using tungsten hexafluoride (WF6), dihydrogen (H2) plasma and dihydrogen sulfide (H2S) based on analyses of the morphology of the WS2crystals. The WS2crystal grain size increases from ∼20 to 200 nm by lowering the nucleation density. This is achieved by lowering the precursor adsorption rate on the starting surface using an inherently less reactive starting surface, by decreasing the H2plasma reactivity, and by enhancing the mobility of the adsorbed species at higher deposition temperature. Since silicon dioxide (SiO2) is less reactive than aluminum oxide (Al2O3), and diffusion and crystal ripening is enhanced at higher deposition temperature, WS2nucleates in an anisotropic island-like growth mode with preferential lateral growth from the WS2crystal edges. This work emphasizes that increasing the crystal grain size while controlling the basal plane orientation is possible during ALD at low deposition temperatures, based on insight in the nucleation behavior, which is key to advance the field of ALD of 2D materials. Moreover, this work demonstrates the conformal deposition on three-dimensional (3D) structures, with WS2retaining the basal plane orientation along topographic structures.